Urea Electrosynthesis from Nitrate and CO₂ on Diatomic Alloys

Advanced Materials, Год журнала: 2024, Номер 36(30)

Опубликована: Июнь 14, 2024

Abstract Urea electrosynthesis from co–electrolysis of NO 3 − and CO 2 (UENC) offers a promising technology for achieving sustainable efficient urea production. Herein, diatomic alloy catalyst (CuPd 1 Rh –DAA), with mutually isolated Pd atoms alloyed on Cu substrate, is theoretically designed experimentally confirmed to be highly active selective UENC catalyst. Combining theoretical computations operando spectroscopic characterizations reveals the synergistic effect –Cu sites promote via tandem catalysis mechanism, where site triggers early C–N coupling promotes *CO –to–*CO NH steps, while facilitates subsequent protonation step *COOHNH toward formation. Impressively, CuPd –DAA assembled in flow cell presents highest Faradaic efficiency 72.1% yield rate 53.2 mmol h −1 g cat at −0.5 V versus RHE, representing nearly performance among all reported catalysts.

Язык: Английский

---

Isolated Metal Centers Activate Small Molecule Electrooxidation: Mechanisms and Applications

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 26, 2025

Abstract Electrochemical oxidation of small molecules shows great promise to substitute oxygen evolution reaction (OER) or hydrogen (HOR) enhance kinetics and reduce energy consumption, as well produce high‐valued chemicals serve fuels. For these reactions, high‐valence metal sites generated at oxidative potentials are typically considered active trigger the process molecules. Isolated atom site catalysts (IASCs) have been developed an ideal system precisely regulate state coordination environment single‐metal centers, thus optimize their catalytic property. The isolated in IASCs inherently possess a positive state, can be more readily homogeneous under than nanoparticle counterparts. Meanwhile, merely centers but lack ensemble sites, which alter adsorption configurations compared with counterparts, induce various pathways mechanisms change product selectivity. More importantly, construction is discovered limit d‐electron back donation CO 2p * orbital overly strong on resolve poisoning problems most electro‐oxidation reactions improve stability. Based advantages fields electrochemical molecules, this review summarizes recent developments advancements focusing anodic HOR fuel cells OER electrolytic alternative such formic acid/methanol/ethanol/glycerol/urea/5‐hydroxymethylfurfural (HMF) key reactions. merits different decoding structure–activity relationships specifically discussed guide precise design structural regulation from perspective comprehensive mechanism. Finally, future prospects challenges put forward, aiming motivate application possibilities for diverse functional IASCs.

Язык: Английский

---

Single-Atom-Alloy Catalysts for Enhanced Hydrogenation Reaction Process: Mechanism, Regulation Strategy, and Design Principle

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 3674 - 3698

Опубликована: Фев. 14, 2025

Язык: Английский

---

Metal–organic framework-derived single-atom catalysts for electrocatalytic energy conversion applications

Journal of Materials Chemistry A, Год журнала: 2024, Номер 12(30), С. 18921 - 18947

Опубликована: Янв. 1, 2024

Single-atom catalysts (SACs) derived from metal–organic frameworks (MOFs) are revolutionizing electrocatalytic energy conversion.

Язык: Английский

---

Radiocatalytic synthesis of acetic acid from CH4 and CO2

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(44)

Опубликована: Июль 26, 2024

Abstract The C−C coupling of methane (CH 4 ) and carbon dioxide (CO 2 to generate acetic acid 3 COOH) represents a highly atom‐efficient chemical conversion, fostering the comprehensive utilization greenhouse gases. However, inherent thermodynamic stability kinetic inertness CH CO present obstacles achieving efficient selective conversion at room temperature. Our study reveals that hydroxyl radicals (⋅OH) hydrated electrons (e aq − produced by water radiolysis can effectively activate , yielding methyl (⋅CH radical anions(⋅CO facilitate production COOH ambient introduction radiation‐synthesized CuO‐anchored TiO bifunctional catalyst could further enhance reaction efficiency selectivity remarkably boosting radiation absorption stability, resulting in concentration 7.1 mmol ⋅ L −1 with near‐unity (>95 %). These findings offer valuable insights for design implementation radiation‐induced conversion.

Язык: Английский

---

Isolated Tin Enhanced CO Coverage‐Regulation on Sn₁Cu Alloy for Selective CO₂ Electroreduction to C₂₊ Products

Small, Год журнала: 2025, Номер unknown

Опубликована: Янв. 15, 2025

Electricity-powered C─C coupling of CO2 represents an attractive strategy for producing valuable commodity chemicals with renewable energy, but it is still challenging to gain high C2+ selectivity at current density. Here, a Sn1Cu single-atom alloy (SAA) reported isolated Sn atom embedded into the Cu lattice, as efficient ectrocatalyst reduction. The prepared Sn1Cu-SAA catalyst shows maximal Faradaic efficiency 79.3% 800 mA cm-2, which can be kept stable least 16 h. combination in situ spectroscopy and DFT calculation reveal that introduced promote activation *CO, enhance CO coverage on Sn1Cu-SAA. As results, reaction barrier pathway significantly reduced, boosting generation products. These findings offer novel sight fabricating multicarbon products from via regulation concentration intermediates catalytic interface.

Язык: Английский

---

The role of the morphological motifs in syngas product selectivity during CO2 photoreduction

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 159711 - 159711

Опубликована: Янв. 1, 2025

Язык: Английский

---

Gold Single Atom Doped Defective Nanoporous Copper Octahedrons for Electrocatalytic Reduction of Carbon Dioxide to Ethylene

ACS Nano, Год журнала: 2025, Номер unknown

Опубликована: Янв. 24, 2025

Electrocatalytic CO2 reduction into high-value multicarbon products offers a sustainable approach to closing the anthropogenic carbon cycle and contributing neutrality, particularly when renewable electricity is used power reaction. However, lack of efficient durable electrocatalysts with high selectivity for multicarbons severely hinders practical application this promising technology. Herein, nanoporous defective Au1Cu single-atom alloy (De-Au1Cu SAA) catalyst developed through facile low-temperature thermal in hydrogen subsequent dealloying process, which shows toward ethylene (C2H4), Faradaic efficiency 52% at current density 252 mA cm–2 under potential −1.1 V versus reversible electrode (RHE). In situ spectroscopy measurements functional theory (DFT) calculations reveal that C2H4 product results from synergistic effect between Au single atoms Cu sites on surface catalysts, where promote *CO generation defects stabilize key intermediate *OCCO, altogether enhances C–C coupling kinetics. This work provides important insights design electrochemical products.

Язык: Английский

---

Catalysis in Sustainable Energy Resources: Overview Studies of Hydrogen, Methane, Biomass and Plastics

Industrial Chemistry and Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

Building a sustainable energy system is currently major challenge. In this review, we introduce catalysis of promising systems, aiming to draw attention development in energy.

Язык: Английский

---

Visible Light‐Driven Acetaldehyde Production from CO₂ and H₂O via Synergistic Vacancies and Atomically Dispersed Cu Sites

Angewandte Chemie International Edition, Год журнала: 2025, Номер unknown

Опубликована: Март 6, 2025

Abstract Acetaldehyde (CH 3 CHO) is of great industrial importance and serves as a key intermediate in various organic transformations. Photocatalytic production acetaldehyde from CO 2 represents sustainable route compared to conventional oxidation processes. However, current photocatalytic systems often face challenges, including limited product selectivity dependence on sacrificial reagents. Here, we present Cd 0.6 Zn 0.4 S (CZS) photocatalyst co‐modified with sulfur vacancies atomically dispersed Cu (Cu/CZS−Vs) for the efficient conversion acetaldehyde. Charge density analysis reveals that induce charge accumulation around adjacent metal atoms, creating active sites strongly anchor H + , thereby promoting while suppressing competing hydrogen evolution reaction. The facilitate intermediates (i.e., *CHO *CO) crucial C *OCCHO, which can subsequently be converted As result, this catalyst achieves an yield 121.5 μmol g −1 h ca. 80 % via absence agents, along quantum efficiency 0.53 at 400 nm, underscoring its potential practical applications. These results are expected pave way future developments green chemical

Язык: Английский

---